AICHE JOURNAL
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2025
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IF 4
Bin Chen,Xingwen Cha,Xuexue Dong,Juanjuan Bian,Jiale Huang,Qingbiao Li,Xiaoqing Huang,Guowu Zhan
Upgrading biomass-derived fatty acids through the H 2 -free and solvent-free catalytic deoxygenation process is both safe and eco-friendly. Herein, we used modified rice husk-derived biochar with ultra-high specific surface area and abundant surface groups as a support to design a homologous bimetallic site catalyst containing Ni single atoms (Ni 1 ) and Ni nanoclusters (Ni n ), the synergy between which is dedicated to excellent catalytic performance. The designed catalyst, Ni 1+n /A-bio-AC, demonstrated an impressive 89.8% selectivity for odd-numbered long-chain alkanes during the H 2 -free and solvent-free deoxygenation of stearic acid, with a turnover frequency value over 18 times higher than conventional Ni/AC. Multiple characterizations revealed the coexistence of Ni 1 and Ni n on the catalyst support. Experimental and theoretical calculations showed that Ni n facilitates the adsorption of fatty acid substrates. While Ni 1 serves as highly dispersed Lewis acid sites, enhancing the dehydrogenation of fatty alcohol intermediates during the in situ hydrodeoxygenation and lowering the decarboxylation pathway energy barriers via electronic synergy with Ni n , thus remarkably boosting the catalytic deoxygenation activity. This work provides a novel Ni dual-site catalyst for developing biomass resource conversion technologies.
研究领域:
催化化学
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生物质能
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Yijian Zhang,Kexin Jiao,Jianliang Zhang,Xiaoyue Fan,Shanchao Gao
The viscosity of Fe C Cr melt affects the mass transfer behavior during steelmaking processes. Reasonable regulation of viscosity can improve production efficiency. There is a close relationship between melt viscosity and structure. Therefore, it is of great theoretical significance to analyze the correlation between viscosity and structure of chromium-containing iron melt for the optimization of the whole metallurgical process. This study experimentally investigated the viscosity of Fe C Cr melt and utilized molecular dynamics simulation to analyze the formation and growth behavior of atomic clusters, revealing the correlation mechanism between structure and viscosity. As the Cr content increased from 11 % to 13 %, the melt viscosity increased by 10.05 %. At a temperature range from 1773 K to 1473 K, the viscosity reached a maximum of 15.5 mPa·s, representing a 40.9 % increase. Simulation results indicated that Cr C clusters within the melt act as intermediaries, connecting with Cr Fe and Fe C clusters to form Fe Cr C clusters. The key influence of increased Cr content on viscosity lies in promoting the generation of Fe Cr C multicomponent clusters, while the key influence of temperature reduction lies in promoting cluster growth. With the increase in Cr content, the number of clusters at 1773 K increased from 154 to 175, and the average volume of clusters increased from 212 Å 3 to 224 Å 3 . When the temperature decreased from 1773 K to 1473 K, the number of clusters increased by 51.2 %, and the average volume of clusters increased by 18.75 %. In comparison, the thermal state change had a greater impact on clusters, where temperature reduction led to rapid cluster growth, reduction of free volume within the melt, and ultimately resulted in increased viscosity due to the combined effects.
研究领域:
冶金学
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材料科学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 15
·8202-8212
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IF 11.9
Feng-Yi Zheng,Ruisong Li,Shibo Xi,Fei Ai,Jike Wang
Iron-based catalysts have demonstrated fascinating activities in the oxygen reduction reaction (ORR), especially due to the synergistic effect between atoms and clusters, but challenging for further improvement. Herein, a strategy is developed to optimize the catalyst with nitrogen-coordinated Fe single atoms (SAs) and closely surrounding Fe atomic clusters (ACs) towards efficient ORR. The FeSA/FeAC-NC 900 delivers excellent ORR activity with half-wave potential (E1/2) in both acidic (0.80 V) and alkaline (0.90 V) media, as well as superior stability. Theoretical calculations further reveal that the synergistic effects of Fe-based SAs and ACs along with porous structures can decrease the overall energy barrier in the ORR process. Besides, the FeSA/FeAC-NC 900-based zinc–air battery manifests a high peak power density (214.3 mW cm−2) and a high-specific capacity (773.6 mA h g−1). This work provides a new perspective to highly optimize the synergistic interaction of SAs and ACs for boosting activity and energy storage.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Xuanbei Peng,Hongfang Cai,Yanliang Zhou,Jun Ni,Xiuyun Wang,Bingyu Lin,Jianxin Lin,Lirong Zheng,Chak-tong Au,Lilong Jiang
Theoretical studies have demonstrated that metal atomic clusters are highly efficient in catalytic ammonia synthesis under mild conditions. However, activation of N2 over atomic clusters from an experimental viewpoint has not been systematically investigated. Here, for the first time, cobalt atomic dimers on a nitrogen–carbon support were synthesized for NH3 synthesis. It is disclosed that N2 activation over Co2 atomic clusters (Co2 ACCs) is entirely different from that over Co single-atom catalysts (Co SACs) or Co nanoparticles (Co NPs). A suite of in situ spectroscopy studies reveal that Co2 ACCs not only provide active sites to promote strong metal–support interactions but also initiate strong interclustering interactions, resulting in electron transfers from Co d-orbitals to antibonding orbitals of N2 molecules. As such, the activation energy of the Co2 ACC catalyst in NH3 synthesis is small. Consequently, the catalytic activity of the developed Ba-promoted Co2 ACC catalyst reached 19.42 mmolNH3 gcat–1 h–1 at 400 °C and 1 MPa, which is much superior than that of other Co-based catalysts under such mild conditions. More importantly, the synthesis strategy of Co2 ACCs has general applicability as demonstrated in the preparation of Fe2 and Mn2 atomic clusters.
研究领域:
催化化学
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材料科学
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物理化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jin Wang,Yefei Chen,Wei Cheng,Hong Li,Meng Liu,Xianmang Xu,Peiyu Zhao,Lixiang Xing,Daijie Wang
Carbon based dual-metal sites materials have garnered considerable attention owing to their atomically dispersed active sites and synergistic effects. However, precise control over the coordination environment and prevention of metal aggregation remain challenging. Herein, we demonstrate a green synthesis of Cu-Fe dual atomic clusters on N-doped porous carbon (CuFe AC@NC) via a chitosan-glutamic acid hydrogel platform. The hydrogel’s amino/hydroxyl/carboxyl groups ensure uniform bimetallic dispersion and inhibit pyrolysis-induced aggregation. Combined experimental and theoretical analyses reveal the distinct roles of Cu and Fe: Fe induces catalytic graphitization for hierarchical pores and enhanced ORR activity, while Cu modulates electronic states and prevents Fe aggregation. The optimized CuFe AC@NC exhibits exceptional ORR activity, and enables Zn-air batteries with a high open-circuit voltage (1.470 V), remarkable specific capacity (806.2 mAh g −1 ), and stable cycling performance. This work provides a green methodology for designing dual-metal-site catalysts and elucidates structure–property relationships, advancing the development of cost-effective energy storage systems.
研究领域:
材料科学
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能源化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
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2024
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IF 6.3
Zhi Song,Xiayan Zhang,Boxia Liu,Jialu Liu,Yeqiong Huang,Dongxu Han,Chuhan Xing
In this study, low-cost coal gasification slag derivative (CGD) was used as a carrier, and highly active Ni atom clusters were successfully loaded on the carrier using the electrostatic self-assembly method to prepare a Ni-CGD composite catalyst. It was used to activate persulfate (PDS) and monopersulfate (PMS) to efficiently remove tetracycline (TC) from aqueous solutions. Experimental results show that Ni-CGD/PDS and Ni-CGD/PMS system exhibits nearly 100 % degradation efficiency for TC between pH 4 and 11. PDS and PMS molecules can be adsorbed on the surface of Ni-CGD materials effectively, and a reaction center with high redox potential can be formed on the catalyst surface through the interaction between molecules. This phenomenon enhances the transfer of electrons from the relatively high-potential functional groups on the TC molecules to the catalyst surface. In addition, the strong interaction between Ni-CGD and the activator promotes the formation of more surface active sites, which can receive electrons from TC molecules, leading to the oxidative degradation of TC. Quenching experiments and EPR tests indicate that direct electron transfer is the main reaction pathway for TC degradation.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
iScience
·
2023
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IF 5.8
Jian Du,Yunxuan Ding,Yu Guo,Licheng Sun,Fei Li
Carbon-supported iron-cobalt bimetallic electrocatalysts usually exhibit robust catalytic activity toward the oxygen evolution reaction (OER). However, the spatial isolation of Fe species at atomic level on cobalt-carbon solid remains a great challenge for practical catalytic applications in the OER. Here, we report the fabrication of CoFe bimetal porous carbon electrocatalysts by pyrolysis of molecularly defined iron complexes such as FePc (Pc = phthalocyanine) and Fe(acac) 3 pre-encapsulated in the cavities of zeolitic imidazolate framework (ZIF)-67. With this unique strategy, high-loading atomic Fe nanoclusters (Fe-ACs) and Fe single atoms (Fe-SAs) were supported on Co/NC hybrids relying on the size of the molecular Fe precursors. The former exhibited superior OER performance to the single Fe atom-decorated Co/NC, as well as other ZIF-67-derived electrocatalysts. Theoretical modulation suggests Co as the OER active site for Fe-ACs@Co/NC at the in situ -formed FeOOH-ACs/Co 3 O 4 interface, while Fe was proposed as the active site for Fe-SAs@Co/NC.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2024
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IF 3.7
Zhijun Wang,Jingjing Wu,Limin Liu,Wenchi Wu,Yinfeng Wang,Haigen Huang,Fei Deng,Xuexia Liu
Currently, platinum (Pt)/carbon support composite materials have tremendous application prospects in the hydrogen evolution reaction (HER). However, one of the primary challenges for boosting their performance is designing a substrate with the desired microstructure. Herein, the intact hollow carbon spheres (HCSs) were prepared via template method. Based on the morphology variation of the as-prepared HCSs-x, we conjectured that the polydopamine (PDA) core was generated first and then slowly grew into a complete overburden (SiO2@PDA). Afterward, Pt atomic clusters were anchored on the outer shells of HCSs-4 to construct composite electrocatalysts (Pty/HCSs-4) by a chemical reduction method. Due to the low charge-transfer resistance, the HCSs have a large electrochemical surface area and provide a continuous electron transport pathway, boosting the atom utilization efficiency during hydrogen production and release. The synthesized Pt2.5/HCSs-4 electrocatalysts exhibit excellent HER activity in acidic media, which can be ascribed to the compositional modulation and delicate structural design. Specifically, when the overpotential is 10 A g–1, the overpotential can achieve 92 mV. This work opens a new route to fabricate Pt-based electrocatalysts and brings a new understanding of the formation mechanism of HCSs.
研究领域:
材料科学
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化学工程
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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Chaochen Wang,Wangxin Ge,Lei Tang,Yanbin Qi,Lei Dong,Hongliang Jiang,Jianhua Shen,Yihua Zhu,Chunzhong Li
ABSTRACT Metal single-atom/atomic cluster catalysts (SA/AC) have emerged as effective electrocatalysts for the CO 2 reduction reaction (CO 2 RR) due to their high metal atom utilization and controllable metal coordination environments. However, the designing and tuning of the local electronic environments of SA/AC ensembles remain a significant challenge. In this work, we develop a single-atom-modified atomic cluster copper catalyst (Cu SA/ACs) for CO 2 RR. The SA/AC-induced modulation of the local electronic structure enhances CO 2 adsorption on the atomic cluster; additionally, the atomic cluster provides abundant active hydrogen for CO 2 protonation by mediating hydrolysis dissociation on the SAs. Consequently, compared to copper single-atom catalysts (Cu SACs), the Cu SA/ACs exhibit significantly improved activity, the current is 3.6 times that of Cu SACs, and the Faradaic efficiency of CO rose from 27.15% to 98.94%. The Cu SA/ACs catalyst can efficiently reduce CO 2 to CO in flow-cell configuration, and the CO selectivity is 93.06% at a current density of 600 mA cm –2 . The maximum energy efficiency of the cathode is 61.9%, which is superior to that of most CO 2 -to-CO catalysts. This work provides a new perspective for developing efficient SA/AC catalysts.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
RARE METALS
·
2025
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IF 11
Wu Jing,Rong Jian,Chen Wang-Yi,Wang Chao-Sheng,Feng Chu-Jun,Ao Huai-Sheng,Zhu Cheng-Zhang,Zhang Yu-Zhe,Li Zhong-Yu
Regulating the electronic structure and oxygen-containing intermediates adsorption behavior on Fe-based catalysts is of great significance to cope with the sluggish oxygen reduction reaction (ORR) kinetics, but it still remains a great challenge. In this work, Fe atom clusters (Fe AC ) modified by high-density Cu single atoms (Cu SA ) in a N,S-doped porous carbon substrate (Fe AC /Cu SA @NCS) is reported for enhanced ORR electrocatalysis. Fe AC /Cu SA @NCS exhibits excellent ORR performance with a half-wave potential ( E 1/2 ) of 0.911 V, a high four-electron process selectivity and excellent stability. The ORR performance is also verified in the Fe AC /Cu SA @NCS-based Zn-air battery, which shows a high peak power density of 192.67 mW cm −2 , a higher specific capacity of 808.3 mAh g −1 and impressive charge–discharge cycle stability. Moreover, density functional theory calculations show that Cu single atoms synergistically modulate the electronic structure Fe active atoms in Fe atomic clusters, reducing the energy barrier of the rate-determining step (i.e., * OH desorption) on Fe AC /Cu SA @NCS. This work provides an effective way to regulate the electronic structure of Fe-based catalysts and optimize their electrocatalytic activity based on the introduction of a second metal source. Graphical abstract
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Tianhua Zhang,Haihui Hu,Jiaxin Li,Yinglong Gao,Lingling Li,Mingyuan Zhang,Xuanbei Peng,Yanliang Zhou,Jun Ni,Bingyu Lin,Jianxin Lin,Bing Zhu,Dongshuang Wu,Linjie Zhang,Lili Han,Lirong Zheng,Xiuyun Wang,Lilong Jiang
Ammonia (NH 3 ) is an excellent candidate for hydrogen storage and transport. However, producing NH 3 under mild conditions is a long-term, arduous task. Atomic cluster catalysts (ACCs) have been shown to be effective for catalytic N 2 -to-NH 3 conversion, opening the door to the development of efficient catalysts under mild conditions. Still, ACC formation with thermally stable catalytic sites remains a challenge because of their high surface free energy . Herein, we report anchoring Ba and/or Ce onto Ru ACCs (2 wt% Ru atomic clusters supported on N-doped carbon) to form so-called clusters–metal oxide promoters electronic interaction (CMEI) to stabilize the Ru atomic clusters. The resulting Ba/Ce/Ru ACCs significantly boost the NH 3 synthesis rate to 56.2 mmol NH3 g cat −1 h −1 at 400 °C and 1 MPa, which is 7.5-fold higher than that of Ru ACC. The strengthened CMEI between the Ba/Ce and Ru atomic clusters across the Ba/Ce/Ru ACC enables electron transfer from Ba and/or Ce to Ru atomic clusters. As such, the electron-enriched Ru atom could facilitate electron transfer to N≡N bond π* orbitals, which would weaken the N≡N bond and drive the eventual conversion of N 2 to NH 3 . This study offers insight into the role of CMEI in Ru ACCs and provides an effective approach for designing stable atomic cluster catalysts for NH 3 synthesis.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2025
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IF 10.5
Huina Sun,Wei Jin,Handong Yao,Mingshi Deng,Xuefeng Wang,Xinghua Gao,Wanyin Xu,Qianqian Li,Yongheng Zhu,Ning Zhao,Yuan Zhang
Helicobacter pylori (H. pylori) is a prevalent bacterium that infects the stomach, can cause numerous gastric diseases, and potentially result in stomach cancer. Current H. pylori detection methods have various limitations; thus, to streamline H. pylori detection, we developed an electrochemical microsensor featuring Ni-based atom cluster (AC)/oxide nanocomposite catalysts for direct biomarker identification. By incorporating Ni ACs and transforming Ni oxides into an ultrathin, porous structure, the resulting material exhibited excellent electrocatalytic activity. In particular, it enabled the detection of urease, a biomarker specific to H. pylori , at concentrations as low as 10 ng/mL. The fabricated Ni AC/NiO@laser-etched graphene (LEG) electrochemical microsensor demonstrated excellent sensitivity and specificity in detecting urease within the concentration range of 10–100 ng/mL. Moreover, its accuracy in analyzing clinical samples matched that of commercial enzyme-linked immunosorbent assay kits, highlighting its potential as a platform for both the personal health monitoring and clinical diagnosis of H. pylori infection. This microsensor exhibited excellent sensitivity and precision and rapid recognition with intuitive operation and ease of use. It holds considerable promise in enhancing and improving medical diagnostics by providing timely and accurate information, enabling earlier interventions, and improving patient outcomes.
研究领域:
医学诊断
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生物传感
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）